Effect of Different Calcination Temperatures on the Structure and Properties of Zirconium-Based Coating Layer Modified Cathode Material Li1.2Mn0.54Ni0.13Co0.13O2

doi:10.1007/s40195-021-01345-8

Abstract

Abstract:

Lithium-rich manganese-based oxides have the advantages of high discharge specific capacity, so they are potential candidates for advanced lithium battery cathode materials. However, they also have drawbacks to be solved such as serious irreversible loss of capacity and voltage decay in the cycling process. Surface coating method was used in this paper to modify the lithium-rich manganese-based oxide (LRMO, Li_1.2Mn_0.54Ni_0.13Co_0.13O₂) to improve its electrochemical properties. Zirconium-based compounds coated LRMO materials (ZBC@LRMO) were obtained via the reaction of lithium hydroxide with zirconium n-butanol and subsequent thermal treatment at different temperatures. The results of X-ray diffraction and transmission electron microscopy confirm that the crystal structure and composition of the ZBC coating layer vary with the calcination temperature. The coating layer obtained at 600 ℃ is composed of tetragonal ZrO₂ and Li₂ZrO₃. The ZBC@LRMO sample with tetragonal ZrO₂ and Li₂ZrO₃ composite exhibits the best electrochemical performance: the discharge capacity of ZBC@LRMO can reach 296 mAh g^-1 at 0.1 C and 120 mAh g^-1 at high rate of 5 C.

Key words: Lithium-ion battery, Cathode material, Zirconium-based compounds coating, Calcination temperature, Electrochemical performance

Zijun Liao, Jiankai Kang, Qi Luo, Caifeng Pan, Jiangdong Chen, Xiaolong Mo, Hanbo Zou, Wei Yang, Shengzhou Chen. Effect of Different Calcination Temperatures on the Structure and Properties of Zirconium-Based Coating Layer Modified Cathode Material Li_1.2Mn_0.54Ni_0.13Co_0.13O₂[J]. Acta Metallurgica Sinica (English Letters), 2022, 35(6): 985-995.

Figures/Tables 14

Table 1 Element compositions (atom ratio) of Li1.2Ni0.13Co0.13Mn0.54O2 (LRMO) and ZBC@LRMO determined by ICP-OES

Sample	Li	Mn	Ni	Co	Zr
LRMO	1.197	0.538	0.133	0.135	0
S1-600	1.130	0.537	0.126	0.128	0.0045

Fig. 1 a XRD patterns of LRMO and 1 wt% ZBO@LRMO, b magnified XRD patterns of samples at the 2θ range of 23°-33°

Table 2 Lattice parameters from the Rietveld refinement of LRMO and ZBC@LRMO

Sample	a (Å)	c (Å)	V (Å³)	c/a	I₍₀₀₃₎/I₍₁₀₄₎
LRMO	2.852924	14.243936	100.402	4.992750	1.4567
S1-400	2.853000	14.242688	100.398	4.992179	1.3180
S1-600	2.852592	14.242246	100.366	4.992738	1.2311
S1-800	2.852008	14.243737	100.336	4.994284	1.2298

Fig. 2 a XRD patterns of 5 wt% ZBO@LRMO calcined at different temperatures, b magnified XRD patterns of samples at the 2θ range of 23°-33°

Fig. 3 XRD patterns of the contrast compound calcined at a 400 ℃, b 600 ℃, c 800 ℃, d Rietveld refinement plot for the Z-600

Fig. 4 SEM images of LRMO and ZBO@LRMO: a LRMO, b S1-400, c S1-600, d S1-800

Fig. 5 a TEM, b HRTEM images of ZBO@LRMO (S1-600)

Fig. 6 a SEM image of S1-600, b energy dispersive spectrum, and c, d, e, f elemental mappings of Ni, Co, Mn, and Zr

Fig. 7 X-ray photoelectron spectra for a Ni 2p, b Co 2p, c Mn 2p, d Zr 3d in pristine LRMO and S1-600 samples

Fig. 8 a Initial charge/discharge curves, b rate performance of samples at various current rates from 0.1 to 5 C, c differential capacity (dQ/dV) plots of first charge/discharge process of pristine and S1-600, d cycling performance and corresponding coulombic efficiency at 1 C of LRMO and S1 samples

Table 3 Initial charge/discharge capacities of LRMO and ZBC@LRMO at 0.1 C rate between 2.0 and 4.8 V

Sample	Charge capacity (mAh g^-1)	Discharge capacity (mAh g^-1)	Irreversible capacity loss (mAh g^-1)	Coulombic efficiency (%)
LRMO	333	265	68	79.6
S1-400	324	272	52	84.1
S1-600	349	296	53	84.8
S1-800	346	283	63	82.0

Fig. 9 Li-ion diffusion coefficient of charging and discharging process: a LRMO and S1-600 charge, b LRMO and S1-600 discharge

Fig. 10 Nyquist plots from the EIS spectra of LRMO and S1-600 after a 5, b 100 cycles at 1 C rate

Table 4 Fitting data of LRMO and S1-600 after 5 and 100 cycles at 1 C rate

	R_ct (Ω)		R_f (Ω)
	After 5 cycles	After 100 cycles	After 5 cycles	After 100 cycles
LRMO	278.7	322.9	66.73	92.12
S1-600	45.75	191.5	29.84	156

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Effect of Different Calcination Temperatures on the Structure and Properties of Zirconium-Based Coating Layer Modified Cathode Material Li_1.2Mn_0.54Ni_0.13Co_0.13O₂

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